Formation of new aerosol particles from trace gases is a major source of cloud condensation nuclei (CCN) in the global atmosphere, with potentially large effects on cloud optical properties and ...Earth's radiative balance. Controlled laboratory experiments have resolved, in detail, the different nucleation pathways likely responsible for atmospheric new particle formation, yet very little is known from field studies about the molecular steps and compounds involved in different regions of the atmosphere. The scarcity of primary particle sources makes secondary aerosol formation particularly important in the Antarctic atmosphere. Here, we report on the observation of ion-induced nucleation of sulfuric acid and ammonia-a process experimentally investigated by the CERN CLOUD experiment-as a major source of secondary aerosol particles over coastal Antarctica. We further show that measured high sulfuric acid concentrations, exceeding 10
molecules cm
, are sufficient to explain the observed new particle growth rates. Our findings show that ion-induced nucleation is the dominant particle formation mechanism, implying that galactic cosmic radiation plays a key role in new particle formation in the pristine Antarctic atmosphere.
Sulphuric acid is a key component in atmospheric new particle formation. However, sulphuric acid alone does not form stable enough clusters to initiate particle formation in atmospheric conditions. ...Strong bases, such as amines, have been suggested to stabilize sulphuric acid clusters and thus participate in particle formation. We modelled the formation rate of clusters with two sulphuric acid and two amine molecules (JA2B2) at varying atmospherically relevant conditions with respect to concentrations of sulphuric acid (H2SO4), dimethylamine (DMA) and trimethylamine (TMA), temperature and relative humidity (RH). We also tested how the model results change if we assume that the clusters with two sulphuric acid and two amine molecules would act as seeds for heterogeneous nucleation of organic vapours (other than amines) with higher atmospheric concentrations than sulphuric acid. The modelled formation rates JA2B2 were functions of sulphuric acid concentration with close to quadratic dependence, which is in good agreement with atmospheric observations of the connection between the particle formation rate and sulphuric acid concentration. The coefficients KA2B2 connecting the cluster formation rate and sulphuric acid concentrations as JA2B2=KA2B2H2SO42 turned out to depend also on amine concentrations, temperature and relative humidity. We compared the modelled coefficients KA2B2 with the corresponding coefficients calculated from the atmospheric observations (Kobs) from environments with varying temperatures and levels of anthropogenic influence. By taking into account the modelled behaviour of JA2B2 as a function of H2SO4, temperature and RH, the atmospheric particle formation rate was reproduced more closely than with the traditional semi-empirical formulae based on sulphuric acid concentration only. The formation rates of clusters with two sulphuric acid and two amine molecules with different amine compositions (DMA or TMA or one of both) had different responses to varying meteorological conditions and concentrations of vapours participating in particle formation. The observed inverse proportionality of the coefficient Kobs with RH and temperature agreed best with the modelled coefficient KA2B2 related to formation of a cluster with two H2SO4 and one or two TMA molecules, assuming that these clusters can grow in collisions with abundant organic vapour molecules. In case this assumption is valid, our results suggest that the formation rate of clusters with at least two of both sulphuric acid and amine molecules might be the rate-limiting step for atmospheric particle formation. More generally, our analysis elucidates the sensitivity of the atmospheric particle formation rate to meteorological variables and concentrations of vapours participating in particle formation (also other than H2SO4).
There is little previous information of the effects of size fractioned particulate air pollution and source specific fine particles (PM(2.5); <2.5 microm) on asthma and chronic obstructive pulmonary ...disease (COPD) among children, adults and the elderly.
To determine the effects of daily variation in levels of different particle size fractions and gaseous pollutants on asthma and COPD by age group.
Levels of particulate air pollution, NO(2) and CO were measured from 1998 to 2004 at central outdoor monitoring sites in Helsinki, Finland. Associations between daily pollution levels and hospital emergency room visits were evaluated for asthma (ICD10: J45+J46) in children <15 years old, and for asthma and COPD (ICD10: J41+J44) in adults (15-64 years) and the elderly (>or=65 years).
Three to 5 day lagged increases in asthma visits were found among children in association with nucleation (<0.03 microm), Aitken (0.03-0.1 microm) and accumulation (0.1-0.29 microm) mode particles, gaseous pollutants and traffic related PM(2.5) (7.8% (95% CI 3.5 to 12.3) for 1.1 microg/m(3) increase in traffic related PM(2.5) at lag 4). Pooled asthma-COPD visits among the elderly were associated with lag 0 of PM(2.5), coarse particles, gaseous pollutants and long range transported and traffic related PM(2.5) (3.9% (95% CI 0.28 to 7.7) at lag 0). Only accumulation mode and coarse particles were associated with asthma and COPD among adults.
Among children, traffic related PM(2.5) had delayed effects, whereas among the elderly, several types of particles had effects that were more immediate. These findings suggest that the mechanisms of the respiratory effects of air pollution, and responsible pollutants, differ by age group.
A dimensionless theory for new particle formation (NPF) was developed, using an aerosol population balance model incorporating recent developments in nucleation rates and measured particle growth ...rates. Based on this theoretical analysis, it was shown that a dimensionless parameter LΓ, characterizing the ratio of the particle scavenging loss rate to the particle growth rate, exclusively determined whether or not NPF would occur on a particular day. This parameter determines the probability that a nucleated particle will grow to a detectable size before being lost by coagulation with the pre-existing aerosol. Cluster-cluster coagulation was shown to contribute negligibly to this survival probability under conditions pertinent to the atmosphere. Data acquired during intensive measurement campaigns in Tecamac (MILAGRO), Atlanta (ANARChE), Boulder, and Hyytiälä (QUEST II, QUEST IV, and EUCAARI) were used to test the validity of LΓ as an NPF criterion. Measurements included aerosol size distributions down to 3 nm and gas-phase sulfuric acid concentrations. The model was applied to seventy-seven NPF events and nineteen non-events (characterized by growth of pre-existing aerosol without NPF) measured in diverse environments with broad ranges in sulfuric acid concentrations, ultrafine number concentrations, aerosol surface areas, and particle growth rates (nearly two orders of magnitude). Across this diverse data set, a nominal value of LΓ=0.7 was found to determine the boundary for the occurrence of NPF, with NPF occurring when LΓ<0.7 and being suppressed when LΓ>0.7. Moreover, nearly 45% of measured LΓ values associated with NPF fell in the relatively narrow range of 0.1
The Station for Measuring Ecosystem–Atmosphere Relations (SMEAR) II is well known among atmospheric scientists due to the immense amount of observational data it provides of the Earth–atmosphere ...interface. Moreover, SMEAR II plays an important role for the large European research infrastructure, enabling the large scientific community to tackle climate- and air-pollution-related questions, utilizing the high-quality long-term data sets recorded at the site. So far, this well-documented site was missing the description of the seasonal variation in aerosol chemical composition, which helps understanding the complex biogeochemical and physical processes governing the forest ecosystem. Here, we report the sub-micrometer aerosol chemical composition and its variability, employing data measured between 2012 and 2018 using an Aerosol Chemical Speciation Monitor (ACSM). We observed a bimodal seasonal trend in the sub-micrometer aerosol concentration culminating in February (2.7, 1.6, and 5.1 µg m−3 for the median, 25th, and 75th percentiles, respectively) and July (4.2, 2.2, and 5.7 µg m−3 for the median, 25th, and 75th percentiles, respectively). The wintertime maximum was linked to an enhanced presence of inorganic aerosol species (ca. 50 %), whereas the summertime maximum (ca. 80 % organics) was linked to biogenic secondary organic aerosol (SOA) formation. During the exceptionally hot months of July of 2014 and 2018, the organic aerosol concentrations were up to 70 % higher than the 7-year July mean. The projected increase in heat wave frequency over Finland will most likely influence the loading and chemical composition of aerosol particles in the future. Our findings suggest strong influence of meteorological conditions such as radiation, ambient temperature, and wind speed and direction on aerosol chemical composition. To our understanding, this is the longest time series reported describing the aerosol chemical composition measured online in the boreal region, but the continuous monitoring will also be maintained in the future.
Ambient aerosol, CCN (cloud condensation nuclei) and hygroscopic properties were measured with a size-segregated CCNC (cloud condensation nuclei counter) in a boreal environment of southern Finland ...at the SMEAR (Station for Measuring Ecosystem-Atmosphere Relations) II station. The instrumental setup operated at five levels of supersaturation S covering a range from 0.1–1% and measured particles with a size range of 20–300 nm; a total of 29 non-consecutive months of data are presented. The median critical diameter Dc ranged from 150 nm at S of 0.1% to 46 nm at S of 1.0%. The median aerosol hygroscopicity parameter κ ranged from 0.41 at S of 0.1% to 0.14 at S of 1.0%, indicating that ambient aerosol in Hyytiälä is less hygroscopic than the global continental or European continental averages. It is, however, more hygroscopic than the ambient aerosol in an Amazon rainforest, a European high Alpine site or a forested mountainous site. A fairly low hygroscopicity in Hyytiälä is likely a result of a large organic fraction present in the aerosol mass comparative to other locations within Europe. A considerable difference in particle hygroscopicity was found between particles smaller and larger than ~100 nm in diameter, possibly pointing out to the effect of cloud processing increasing κ of particles > 100 nm in diameter. The hygroscopicity of the smaller, ~50 nm particles did not change seasonally, whereas particles with a diameter of ~150 nm showed a decreased hygroscopicity in the summer, likely resulting from the increased VOC emissions of the surrounding boreal forest and secondary organic aerosol (SOA) formation. For the most part, no diurnal patterns of aerosol hygroscopic properties were found. Exceptions to this were the weak diurnal patterns of small, ~50 nm particles in the spring and summer, when a peak in hygroscopicity around noon was observed. No difference in CCN activation and hygroscopic properties was found on days with or without atmospheric new particle formation. During all seasons, except summer, a CCN-inactive fraction was found to be present, rendering the aerosol of 75–300 nm in diameter as internally mixed in the summer and not internally mixed for the rest of the year.
High Natural Aerosol Loading over Boreal Forests Tunved, P; Hansson, H.-C; Kerminen, V.-M ...
Science (American Association for the Advancement of Science),
04/2006, Letnik:
312, Številka:
5771
Journal Article
Recenzirano
Aerosols play a key role in the radiation balance of the atmosphere. Here, we present evidence that the European boreal region is a substantial source of both aerosol mass and aerosol number. The ...investigation supplies a straightforward relation between emissions of monoterpenes and gas-to-particle formation over regions substantially lacking in anthropogenic aerosol sources. Our results show that the forest provides an aerosol population of 1000 to 2000 particles of climatically active sizes per cubic centimeter during the late spring to early fall period. This has important implications for radiation budget estimates and relevancy for the evaluation of feedback loops believed to determine our future climate.
Reliable characterization of particles freshly emitted from the ocean surface requires a sampling method that is able to isolate those particles and prevent them from interacting with ambient gases ...and particles. Here we report measurements of particles directly emitted from the ocean using a newly developed in situ particle generator (Sea Sweep). The Sea Sweep was deployed alongside R/V Atlantis off the coast of California during May of 2010. Bubbles were generated 0.75 m below the ocean surface with stainless steel frits and swept into a hood/vacuum hose to feed a suite of aerosol instrumentation on board the ship. The number size distribution of the directly emitted, nascent particles had a dominant mode at 55–60 nm (dry diameter) and secondary modes at 30–40 nm and 200–300 nm. The nascent aerosol was not volatile at 230°C and was not enriched in SO4=, Ca++, K+, or Mg++above that found in surface seawater. The organic component of the nascent aerosol (7% of the dry submicrometer mass) volatilized at a temperature between 230 and 600°C. The submicrometer organic aerosol characterized by mass spectrometry was dominated by non‐oxygenated hydrocarbons. The nascent aerosol at 50, 100, and 145 nm dry diameter behaved hygroscopically like an internal mixture of sea salt with a small organic component. The CCN/CN activation ratio for 60 nm Sea Sweep particles was near 1 for all supersaturations of 0.3 and higher indicating that all of the particles took up water and grew to cloud drop size. The nascent organic aerosol mass fraction did not increase in regions of higher surface seawater chlorophyll but did show a positive correlation with seawater dimethylsulfide (DMS).
Key Points
The ocean is a source of sub 100nm particles to the atmosphere
Hygroscopically the particles behave like an internal mixture of sea salt/organic
Organic mass fraction did not correlate with chlorophyll
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